金刚石材料n-type掺杂相关研究
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摘要
金刚石由于其优异的物理化学性质引起了人们的关注。它在高新科技领域，特别是在高温，高频，大功率电子器件等方面有着极为重要的应用。正是由于具有特殊的物理、化学性质，它在一般的工业制造，热力学器件，光学器件，军事等领域有极大的应用潜力。由于天然金刚石非常稀少，价格昂贵，其应用研究受到很大限制。随着科学技术的发展，CVD技术(化学气相沉积技术)合成金刚石薄膜的成功，使金刚石半导体材料有可能成为新一代半导体芯片材料(既导热又绝缘)，因而超大规模和超高速集成电路的发展可进入一个崭新时代。
与其它半导体材料一样，金刚石作为基本的半导体材料，首先需要实现的就是p-n结，具体说就是能够合成p-型和n-型导电材料。实验发现，天然的杂质金刚石具有p-型导电性，通过CVD生长法或者离子注入法向金刚石中掺入B(硼)离子得到的金刚石p-型导电材料也已实现产业化。但金刚石有效n-型导电材料的研究和制备仍是目前的难点之一。金刚石n-型材料的缺少，限制了金刚石材料电子器件的开发和应用。因而，人们在金刚石n-型材料的研究方面作了大量的理论和实验工作。目前，主要可以分为两种途径：(1)通过掺杂，如Ⅰ、Ⅴ族元素掺杂，B-P(硼—磷)，B-S(硼—硫)共掺杂等，由于各种原因，效果均不理想，不能达到器件化的要求。(2)最近(2003．7)法国科学家Teukam与其研究小组通过对掺硼p-型材料的氘化得到了具有较低激发能量(230meV)的n-型导电薄膜。为金刚石电子器件的研究开发带来了突破性的机遇，有可能基本上解决了n-型金刚石材料的制备问题，对金刚石半导体高性能器件的发展具有深远意义，为金刚石的n-型掺杂研究开辟了一条新思路。但是这种获得n-型导电材料的方法仍有诸多问题需要进一步研究，如：施主能级形成机理及稳定存在的条件等。本文正是针对这些问题开展理论和实验研究的。
基于以上考虑，我们做了以下几方面的工作：
一、利用DFT(密度泛函理论)研究了各种掺杂剂(如H、P、S和B等)对金刚石材料电子性质的影响；不同B-H复合物对氢化金刚石材料能带结构的影响以及对金刚石材料p-n型转化机理进行了分析和讨论。
二、在理论研究的基础上，利用我国生长的high power DF arc plasma jet
Diamond is of attractiveness as a material because of its outstanding physical and chemical properties. It has been associated with a broad range of applications in advanced scientific and technological fields, especially in those of high temperature, high frequency and large power electronic devices. However, its application is limited due to the rarity of natural diamond . With the rapid development of science and technology in recent years, synthetic diamond has been successfully grown by chemical vapor deposition and can be a candidate as a new semiconductor chip material due to its excellent properties, which probably leads to a breakthrough and a new era coming in the development of the SLS1 (Super Large Scale Integrated circuits) .
Diamond as a basic semiconductor material, just like others, is needed for n-type conduction as well as its p-type counterpart. It is experimentally discovered that the natural diamond is of p-type characteristic, and the CVD p-type diamond can be also obtained and has been industrialized. However, so far the efficient n-type diamond remains unavailable, which hampers its application and exploitation in electronic devices fields. Great efforts have been made both theoretically and experimentally to obtain available n-type diamond materials. There are two methods to obtain n-type diamond: one way is doping with dopants, such as the elements of I, V group, or co-doping with boron-phosphorous and boron-sulfur and so on. However, the results are not available. The other method is that B-doped p-type diamond can be transformed to n-type diamond after deuteration, which is recently reported by Teukam et al (in July 2003). This method may offer a new opportunity for obtaining n-type diamond and resolve its preparation completely. But many problems are needed to investigate, such as the formation mechanism and stability of the donor
与其它半导体材料一样，金刚石作为基本的半导体材料，首先需要实现的就是p-n结，具体说就是能够合成p-型和n-型导电材料。实验发现，天然的杂质金刚石具有p-型导电性，通过CVD生长法或者离子注入法向金刚石中掺入B(硼)离子得到的金刚石p-型导电材料也已实现产业化。但金刚石有效n-型导电材料的研究和制备仍是目前的难点之一。金刚石n-型材料的缺少，限制了金刚石材料电子器件的开发和应用。因而，人们在金刚石n-型材料的研究方面作了大量的理论和实验工作。目前，主要可以分为两种途径：(1)通过掺杂，如Ⅰ、Ⅴ族元素掺杂，B-P(硼—磷)，B-S(硼—硫)共掺杂等，由于各种原因，效果均不理想，不能达到器件化的要求。(2)最近(2003．7)法国科学家Teukam与其研究小组通过对掺硼p-型材料的氘化得到了具有较低激发能量(230meV)的n-型导电薄膜。为金刚石电子器件的研究开发带来了突破性的机遇，有可能基本上解决了n-型金刚石材料的制备问题，对金刚石半导体高性能器件的发展具有深远意义，为金刚石的n-型掺杂研究开辟了一条新思路。但是这种获得n-型导电材料的方法仍有诸多问题需要进一步研究，如：施主能级形成机理及稳定存在的条件等。本文正是针对这些问题开展理论和实验研究的。
基于以上考虑，我们做了以下几方面的工作：
一、利用DFT(密度泛函理论)研究了各种掺杂剂(如H、P、S和B等)对金刚石材料电子性质的影响；不同B-H复合物对氢化金刚石材料能带结构的影响以及对金刚石材料p-n型转化机理进行了分析和讨论。
二、在理论研究的基础上，利用我国生长的high power DF arc plasma jet
Diamond is of attractiveness as a material because of its outstanding physical and chemical properties. It has been associated with a broad range of applications in advanced scientific and technological fields, especially in those of high temperature, high frequency and large power electronic devices. However, its application is limited due to the rarity of natural diamond . With the rapid development of science and technology in recent years, synthetic diamond has been successfully grown by chemical vapor deposition and can be a candidate as a new semiconductor chip material due to its excellent properties, which probably leads to a breakthrough and a new era coming in the development of the SLS1 (Super Large Scale Integrated circuits) .
Diamond as a basic semiconductor material, just like others, is needed for n-type conduction as well as its p-type counterpart. It is experimentally discovered that the natural diamond is of p-type characteristic, and the CVD p-type diamond can be also obtained and has been industrialized. However, so far the efficient n-type diamond remains unavailable, which hampers its application and exploitation in electronic devices fields. Great efforts have been made both theoretically and experimentally to obtain available n-type diamond materials. There are two methods to obtain n-type diamond: one way is doping with dopants, such as the elements of I, V group, or co-doping with boron-phosphorous and boron-sulfur and so on. However, the results are not available. The other method is that B-doped p-type diamond can be transformed to n-type diamond after deuteration, which is recently reported by Teukam et al (in July 2003). This method may offer a new opportunity for obtaining n-type diamond and resolve its preparation completely. But many problems are needed to investigate, such as the formation mechanism and stability of the donor
引文
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1. A. M. Zaitsev, Optical Properties of Diamond: a Data Handbook, Springer-Verlag, Berlin, (2001) 389
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10．肖慎修，王崇愚，陈天朗，密度泛函理论的离散变分方法在化学和材料物理学中的应用，(1998)12
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34. Kalish R, Reznik A, Uzan-Saguy C et al. ,Appl. Phys. Lett., 76(2000) 757
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38. Briddon PR, Jones R, Lister GMS., J Phys. C, 21 (1988) L1027
39. Nebel C., Nat. Mater., 2 (2003) 431
40. Chevallier J, Lusson A, Theys B et al., Diamond Relat. Mater., 8 (1999) 278
1. Chia-Fu Chen, Hui-Chen Hsieh, Diamond and Related Materials, 9 (2000) 125
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24. Zéphirin Teukam, Jacques Chevallier et al., Nature Materials, 12 (2003) 482
25．离子注入原理与技术，北京市辐射中心．北京师范大学低能核物理研究所离编，124
2. Z. Remes, C. Uzan-Saguy, E. Baskin et al., Diamond ahd Related Materials, 13 (2004) 713
3. E. Gheeraert, Ncasanova, A. Tajani et al., Diamond and Related Materials, 11 (2002) 289
4．戴达煌，金刚石薄膜沉积工艺与应用，北京冶金工业出版社，194
5. S.A. Kajihara, A. Antonelli, J. Bernhole et al., Phys. Rev. Lett., 66(1991) 2010
6. Zvanut ME, Carlos WE, Freitas Jr. JA et al., Appl. Phys. Lett., 65 (1994) 2287
7. Prawer S, Jamieson DN, Walker RJ Lee KK et al., Diamond Film Technol, 6 (1996) 351
1. A. M. Zaitsev, Optical Properties of Diamond: a Data Handbook, Springer-Verlag, Berlin, (2001) 389
2. W.J.P. Van Enckevort, Synthetic Diamond: Emerging CVD Science and Technology, (1994) 322
3. J.I. Pankove, C. H. Qiu, Synthetic Diamond: Emerging CVD Science and Technology, (1994) 403
4. J. Walker, Rep. Prog., Phys., 42 (1979) 1605.
5. A.T. Collins, E.C. Lightowlers, Phys. Rev., 171/3 (1968) 843
6．陈光华，张阳，金刚石薄膜的制备与应用，(2004)
7. Dischler, Wild. Low-pressure synthetic Diamond, Springer (1998)
8. Füner, M., Wild, C., Koidl, P., Appl. Phys. Lett., 72 (1998) 1149
9. Füner M., Wild C., Koidl P., Surf. Coat. Techno, 116～119 (1999) 853
10. Gildenblat, G. Sh., S. A. Grot et al., Proc. IEEE 79, 5 (1991) 647
11. Johan F. Prins, Physics Review B, 38 (1988) 5576
12. F. Fontaine, C. Uzan-Saguy, B. Philosoph et al., Appl. Phys. Let., 68 (1996) 2264
13. Vogel Thomas, Meijer Jan, Zaitsev et al., Diamond and Related Materials, 13 (2004) 1822
14. Kajihara SA, Antonelli A, Bernholc et al., Phys. Rev. Lett., 66(1991)2010
15. Zvanut ME, Carlos WE, Freitas Jr. JA et al., Appl. Phys. Lett., 65(1994)2287
16. Prawer S, Jamieson DN, Walker RJ Lee KK et al., Diamond Film Technol., 6(1996)351
17. A.T. Collins, Properties and Growth of Diamond, INSPEC (1994) 284
18. G. Braunstein, R. Kalish, Appl. Phys. Lett., 38 (1981) 416
19. S. Prawer, D.N. Jamieson, R.J. Walker et al., Diamond Films and Technology (1996), in press
20. J. F. Prins, Diamond Film. Technol. 8/4 (1998) 181
21. Prins J. F., Phys. Rev. B.,61 (1999) 7191
22. X.J.Hu, R.B.Li, H. S. Shen et al., Carbon, 42(2004)1501
23. Rongbin Li, Xiaojun Hu, Hesheng Shen et al., Materials Letters, 58(2004)1835
24. Zephirin Teukam, Jacques, Chevallier et al., Nature Materials, 12(2003)482
25. Koizumi S., Teraji T., Kanda H., Diamond and Related Materials, 9 (2000) 935
1. P. Hohenberg, W. Kohn, Phys. Rev. B, 136 (1964) 864
2. Kohn W., Sham, L. J., Phys. Rev. A, 140(1965) 1133
3. D.M. Ceperley, B. J. Alder, Phys. Rev. Lett., 45 (1980) 566
4. J.P. Perdew, Physica. B, 172 (1991) 1
5. J.P. Perdew, A. Zunger, Phys. Phys. B., 23 (1981) 5048
6. S.H. Vosko, L. Wilk, M. Nusair, Can. J. Phys., 58 (1980) 1200
7. H. Stoll, C.M.E. Pavlidou et al., Theor. Chim. Acta, 49 (1978) 143
8. L. Kleinman, S. lee, Phys. Rev. B, 37 (1988) 4684
9. D.C. Langreth, J. P. Perderw. Phys., Rev. B, 21 (1980) 5469
10．肖慎修，王崇愚，陈天朗，密度泛函理论的离散变分方法在化学和材料物理学中的应用，(1998)12
11. Y. Asada, K. Terakura, Phys. Rev, B, 46 (1992) 13599
12. Arssterdam Density Functional (ADF2003), Department of theoretical Chemistry, Vrije Universities, De Boelelaan Amsterdam, The Netherlands (2003)
13. S.H. Vosko, L. Wilk, M. Nusair. Can. J. Phys., 58 (1980) 1200
14. A. D. Becke. Phys. Rev. A., 389(1988)3098
15. J. P. Perdew, Y. Wang., Phys. Rev. B., 33(1986)8800
16. Kresse G, Hafner J., Phys Rev B, 47(1993)558
17. Kresse G, Hafner J., Phys Rev B, 49(1994)14251
18. Kresse G, Furthmuller J., comput mater sci, 6(1996)15
19. Kresse G, Furthmuller J., Phys Rev B, 54(1996)11169
20. Monkhorst Hj, Pack JD., Phys Rev B, 13(1976)5188
21. Vanderbilt D., Phys Rev B, 41(1990)7892
22. Perdew Jp, Chevary JA, et al., Phys Rev B, 46(1992)6671
23. D. P. Erchak, A. G. Ulyashin, R. B. Gelfand et al., Phys. Res. B, 69(1992) 271
24. .R. D. Johnson, R. A. Street, R. L. Thornton, Phys. Rev. B, 33 (1986) 1102
25. J. Chevallier, W. C. Dautremont-Smith, C. W. Tu et al., Appl. Phys. Lett., 47 (1985) 108
26. J.P. Goss, R. Jones, M. I. Heggie et al., Phys.Rev. B, 65 (2002) 115207
27. S.P. Mehandru, A. B. Anderson, J. Mater. Res., 9 (1994) 383
28. Goss JP, Jones R, Heggie MI, et al., Phys. Rev. B , 35(2002) 115207-1
29. S. A. Kajihara, A. Antonelli, J. Bernholc et al., Phys. Rev. Lett., 66 (1991)2010
30. Y.Dai, S.Han, B.Huang et al., Mater.Sci. Eng. B, 99(2003)531
31. J.P. Goss, R. Jones, M. I. Heggie et al., Phys. Rev. B, 65 (2002) 115207
32. T.Nishimatsu, H. Katayama-Yoshida, N. Orita. , Physica B, 302 (2001) 149
33. Sakaguchi I et al., Phys. Rev. B, 60 (1999) R2139 - 41.
34. Kalish R, Reznik A, Uzan-Saguy C et al. ,Appl. Phys. Lett., 76(2000) 757
35. Miyazaki T, Okushi H., Diamond Relat. Mater., 11(2002) 323
36. Saada D, Adler J, Kalish R., Appl. Phys. Lett., 77(2000)878
37. Teukam Z, Chevallier J, Saguy C et al., Nat. Mater., 2(2003)482
38. Briddon PR, Jones R, Lister GMS., J Phys. C, 21 (1988) L1027
39. Nebel C., Nat. Mater., 2 (2003) 431
40. Chevallier J, Lusson A, Theys B et al., Diamond Relat. Mater., 8 (1999) 278
1. Chia-Fu Chen, Hui-Chen Hsieh, Diamond and Related Materials, 9 (2000) 125
2. Ying Dai, Dadi Dai, Donghong Liu et al., Appl. Phys. Lett., 84 (2004) 1895
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25．离子注入原理与技术，北京市辐射中心．北京师范大学低能核物理研究所离编，124